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Data repository for "Disentangling the Evolution of Electrons and Holes in photoexcited ZnO nanoparticles", submitted to Structural Dynamics (#SDY23-AR-XAS2023-00063). Data are divided in 4 numbered folders, organized as follows: Folder "1 - ZnO_PL_scans": This folder contains the raw data of ultrafast photoluminescence measurement. ZnO_full_time.pxp file (Igor Pro by WaveMetrics) is the ultrafast photoluminescence(PL) data obtained upon pumping at 4.66eV at different fluence :0.8, 2.3, 4.7, 5.4 (unit: mJ*cm-2), which are plotted in Figure 1, Figure 2, Figure S3, Figure S4, and Figure S5. time_0312cuts.txt, zno1812corr_wn_233nm.txt, PL_cut_fit2exp.ipynb are the time delay, time trace cut at PL peak, and python code for exponential fitting, respectively, which is plotted in Figure S7. ZnO Raman_rise.pxp contains the Raman data of water in comparison of rising of ZnO PL data, which is plotted in Figure S6. Folder "2 - ZnO_XANES_transient": This folder contains the raw data of Zn K-edge fs-XANES transients data measured in SACLA (2ps), which are plotted in Figure 3 and Figure 4. In the SACLA_APS_comparison_XANES.txt file: the headers "allDiff_N", "allscaler1S3_N", "fluonorm_diff_norm", indicates the transient data measured in APS (100ps), ground-state XAS, and the transient fs-XANES data measured in SACLA(2ps), repectively. Folder "3 - ZnO_XANES_timescan":This folder contains the fs-XANES time scan along with the fitting python code, which is plotted in Figure 5 and Figure S8. Folder "4 - ZnO_MD_Simulation" - This folder contains the result of ab-initio molecular dynamics simulations, which is plotted in Figure 6.

We present the first lasing results of SwissFEL, a hard X-ray free-electron laser (FEL) that recently came into operation at the Paul Scherrer Institute in Switzerland. SwissFEL is a very stable, compact and cost-effective X-ray FEL facility driven by a low-energy and ultra-low-emittance electron beam travelling through short-period undulators. It delivers stable hard X-ray FEL radiation at 1-A wavelength with pulse energies of more than 500 μJ, pulse durations of ~30 fs (root mean square) and spectral bandwidth below the per-mil level. Using special configurations, we have produced pulses shorter than 1 fs and, in a different set-up, broadband radiation with an unprecedented bandwidth of ~2%. The extremely small emittance demonstrated at SwissFEL paves the way for even more compact and affordable hard X-ray FELs, potentially boosting the number of facilities worldwide and thereby expanding the population of the scientific community that has access to X-ray FEL radiation. The first lasing results at SwissFEL, an X-ray free-electron laser, are presented, highlighting the facility’s unique capabilities. A general comparison to other major facilities is also provided.

Long-wavelength pulses from the Swiss X-ray free-electron laser (XFEL) have been used for de novo protein structure determination by native single-wavelength anomalous diffraction (native-SAD) phasing of serial femtosecond crystallography (SFX) data. In this work, sensitive anomalous data-quality indicators and model proteins were used to quantify improvements in native-SAD at XFELs such as utilization of longer wavelengths, careful experimental geometry optimization, and better post-refinement and partiality correction. Compared with studies using shorter wavelengths at other XFELs and older software versions, up to one order of magnitude reduction in the required number of indexed images for native-SAD was achieved, hence lowering sample consumption and beam-time requirements significantly. Improved data quality and higher anomalous signal facilitate so-far underutilized de novo structure determination of challenging proteins at XFELs. Improvements presented in this work can be used in other types of SFX experiments that require accurate measurements of weak signals, for example time-resolved studies., IUCrJ, 7 (6), ISSN:2052-2525

International audience; The Bernina instrument at the SwissFEL Aramis hard X-ray free-electron laser is designed for studying ultrafast phenomena in condensed matter and material science. Ultrashort pulses from an optical laser system covering a large wavelength range can be used to generate specific non-equilibrium states, whose subsequent temporal evolution can be probed by selective X-ray scattering techniques in the range 2–12 keV. For that purpose, the X-ray beamline is equipped with optical elements which tailor the X-ray beam size and energy, as well as with pulse-to-pulse diagnostics that monitor the X-ray pulse intensity, position, as well as its spectral and temporal properties. The experiments can be performed using multiple interchangeable endstations differing in specialization, diffractometer and X-ray analyser configuration and load capacity for specialized sample environment. After testing the instrument in a series of pilot experiments in 2018, regular user operation begins in 2019.

The characterization and commissioning of the X-ray photon single-shot spectrometer (PSSS) at the Aramis beamline of SwissFEL is presented. The device delivers online, non-invasive, high-resolution single-shot measurements of spectral profiles between 4 and 13 keV., The performance and parameters of the online photon single-shot spectrometer (PSSS) at the Aramis beamline of the SwissFEL free-electron laser are presented. The device operates between the photon energies 4 and 13 keV and uses diamond transmission gratings and bent Si crystals for spectral measurements on the first diffraction order of the beam. The device has an energy window of 0.7% of the median photon energy of the free-electron laser pulses and a spectral resolution (full width at half-maximum) ΔE/E on the order of 10−5. The device was characterized by comparing its performance with reference data from synchrotron sources, and a parametric study investigated other effects that could affect the reliability of the spectral information.

Stochastic processes are highly relevant in research fields as different as neuroscience, economy, ecology, chemistry, and fundamental physics. However, due to their intrinsic unpredictability, stochastic mechanisms are very challenging for any kind of investigations and practical applications. Here we report the deliberate use of stochastic X-ray pulses in two-dimensional spectroscopy to the simultaneous mapping of unoccupied and occupied electronic states of atoms in a regime where the opacity and transparency properties of matter are subject to the incident intensity and photon energy. A readily transferable matrix formalism is presented to extract the electronic states from a dataset measured with the monitored input from a stochastic excitation source. The presented formalism enables investigations of the response of the electronic structure to irradiation with intense X-ray pulses while the time structure of the incident pulses is preserved., Free electron X-ray laser pulses, generated by self-amplified spontaneous emission, are stochastic in nature. Here the authors present a reconstruction method for 2D spectroscopy while preserving the intrinsic properties of the incident pulses and apply it to a study towards X-ray intensity induced effects.

The SwissFEL soft X-ray free-electron laser (FEL) beamline Athos will be ready for user operation in 2021. Its design includes a novel layout of alternating magnetic chicanes and short undulator segments. Together with the APPLE X architecture of undulators, the Athos branch can be operated in different modes producing FEL beams with unique characteristics ranging from attosecond pulse length to high-power modes. Further space has been reserved for upgrades including modulators and an external seeding laser for better timing control. All of these schemes rely on state-of-the-art technologies described in this overview. The optical transport line distributing the FEL beam to the experimental stations was designed with the whole range of beam parameters in mind. Currently two experimental stations, one for condensed matter and quantum materials research and a second one for atomic, molecular and optical physics, chemical sciences and ultrafast single-particle imaging, are being laid out such that they can profit from the unique soft X-ray pulses produced in the Athos branch in an optimal way., Journal of Synchrotron Radiation, 26 (4), ISSN:0909-0495, ISSN:1600-5775

The biological influence of radiation on living matter has been studied for years; however, several questions about the detailed mechanism of radiation damage formation remain largely unanswered. Among all biomolecules exposed to radiation, DNA plays an important role because any damage to its molecular structure can affect the whole cell and may lead to chromosomal rearrangements resulting in genomic instability or cell death. To identify and characterize damage induced in the DNA sugar-phosphate backbone, in this work we performed x-ray absorption spectroscopy at the P K-edge on DNA irradiated with either UVA light or protons. By combining the experimental results with theoretical calculations, we were able to establish the types and relative ratio of lesions produced by both UVA and protons around the phosphorus atoms in DNA.

In liquid phase chemistry dynamic solute-solvent interactions often govern the path, ultimate outcome, and efficiency of chemical reactions. These steps involve many-body movements on subpicosecond time scales and thus ultrafast structural tools capable of capturing both intramolecular electronic and structural changes, and local solvent structural changes are desired. We have studied the intra- and intermolecular dynamics of a model chromophore, aqueous [Fe(bpy)3](2+), with complementary X-ray tools in a single experiment exploiting intense XFEL radiation as a probe. We monitored the ultrafast structural rearrangement of the solute with X-ray emission spectroscopy, thus establishing time zero for the ensuing X-ray diffuse scattering analysis. The simultaneously recorded X-ray diffuse scattering patterns reveal slower subpicosecond dynamics triggered by the intramolecular structural dynamics of the photoexcited solute. By simultaneous combination of both methods only, we can extract new information about the solvation dynamic processes unfolding during the first picosecond (ps). The measured bulk solvent density increase of 0.2% indicates a dramatic change of the solvation shell around each photoexcited solute, confirming previous ab initio molecular dynamics simulations. Structural changes in the aqueous solvent associated with density and temperature changes occur with ∼1 ps time constants, characteristic for structural dynamics in water. This slower time scale of the solvent response allows us to directly observe the structure of the excited solute molecules well before the solvent contributions become dominant.

The potential of two-color resonant and degenerate four-wave mixing spectroscopy for investigations of the complex spectra of transition metal dimers is explored. Two-color resonant and degenerate four-wave mixing spectroscopy scans of the well-known A-X and B-X transitions in Cu2 are reported and compared with previous experimental data obtained from standard single-resonance techniques. The selectivity of the method is shown to enable the measurement of isotopologue pure spectra without the need for isotopically enriched metal targets. Specific subsets of the rovibronic structure are separated in a congested spectral region of overlapping transitions. The sensitivity of the method compares satisfactorily with linear spectroscopic methods such as laser-induced fluorescence and cavity ring-down. A new laser vaporization source for the production of transition metal dimers and clusters has been constructed. The new design aims for a high number density and maximum possible shot-to-shot stability. The possibilities of further applications of non-linear four-wave mixing spectroscopy to Cu2 and other transition metal dimers are discussed. Copyright © 2015 John Wiley & Sons, Ltd.

Next generation X ray sources based on the X ray Free Electron Laser (XFEL) concept will provide highly coherent ultrashort pulses of soft and hard X rays with peak intensity many orders of magnitude higher than that of a synchrotron. These pulses will allow studies of femtosecond dynamics at nanometer resolution and with chemical selectivity. They will produce diffraction images of organic and inorganic nanostructures without deleterious effects of radiation damage. © Schweizerische Chemische Gesellschaft.

Past decades have shown the impact of structural information derived from complexes of drug candidates with their protein targets to facilitate the discovery of safe and effective medicines. Despite recent developments in single particle cryo-electron microscopy, X-ray crystallography has been the main method to derive structural information. The unique properties of X-ray free electron laser (XFEL) with unmet peak brilliance and beam focus allow X-ray diffraction data recording and successful structure determination from smaller and weaker diffracting crystals shortening timelines in crystal optimization. To further capitalize on the XFEL advantage, innovations in crystal sample delivery for the X-ray experiment, data collection and processing methods are required. This development was a key contributor to serial crystallography allowing structure determination at room temperature yielding physiologically more relevant structures. Adding the time resolution provided by the femtosecond X-ray pulse will enable monitoring and capturing of dynamic processes of ligand binding and associated conformational changes with great impact to the design of candidate drug compounds.

We present a theoretical analysis for the K- and L-2/3-edge static and picosecond X-ray absorption spectra of [Fe(bpy)(3)](2+). Simulations of the pre-edge region at the Fe K-edge using time-dependent density functional theory demonstrate the importance of Hartree-Fock exchange within the exchange-correlation functional, especially when describing charge transfer and 1s -> 3d transitions. This becomes particularly relevant for range separated functionals, for which the incorporation of Hartree-Fock exchange at short range decreases the absolute error in the excitation energy usually observed using TD-DFT. Finally, we compute and interpret the L-2/3-edge spectrum using the Restricted Open-Shell Configuration Interaction Singles method. (C) 2013 Elsevier B.V. All rights reserved.

We present an ab initio Born-Oppenheimer molecular dynamics study of the early time solvent dynamics after electron abstraction from aqueous iodide. An initial response occurs within ∼75 fs, corresponding to a water molecule sharing almost one electron with the iodine. This is followed by the formation of a transient I0⋯OH2 complex within ∼500 fs. Further insight into the driving forces for this complex are obtained using an energy decomposition analysis and frequency calculations of small clusters. It is shown that the anisotropic solvation shell structure of iodide before electron abstraction is likely to be an important factor in the formation of the complex.

Steady-state and picosecond time-resolved X-ray absorption spectroscopy is used to study the ground and lowest triplet states of [ReX(CO)(3)(bpy)](n+), X = Etpy (n = 1), Cl, or Br (n = 0). We demonstrate that the transient spectra at both the Re L(3)- and Br K-edges show the emergence of a pre-edge feature, absent in the ground-state spectrum, which is associated with the electron hole created in the highest occupied molecular orbital following photoexcitation. Importantly, these features have the same dynamics, confirming previous predictions that the low-lying excited states of these complexes involve a two-center charge transfer from both the Re and the ligand, X. We also demonstrate that the DFT optimized ground and excited structures allow us to reproduce the experimental XANES and EXAFS spectra. The ground-state structural refinement shows that the Br atom contributes very little to the latter, whereas the Re-C-O scattering paths are dominant due to the so-called focusing effect. For the excited-state spectrum, the Re-X bond undergoes one of the largest changes but still remains a weak contribution to the photoinduced changes of the EXAFS spectrum.

Nature Communications 7, 12314(2016). doi:10.1038/ncomms12314, Serial femtosecond crystallography (SFX) using X-ray free-electron laser sources is an emerging method with considerable potential for time-resolved pump-probe experiments. Here we present a lipidic cubic phase SFX structure of the light-driven proton pump bacteriorhodopsin (bR) to 2.3 Å resolution and a method to investigate protein dynamics with modest sample requirement. Time-resolved SFX (TR-SFX) with a pump-probe delay of 1 ms yields difference Fourier maps compatible with the dark to M state transition of bR. Importantly, the method is very sample efficient and reduces sample consumption to about 1 mg per collected time point. Accumulation of M intermediate within the crystal lattice is confirmed by time-resolved visible absorption spectroscopy. This study provides an important step towards characterizing the complete photocycle dynamics of retinal proteins and demonstrates the feasibility of a sample efficient viscous medium jet for TR-SFX., Published by Nature Publishing Group, London

A wavefront metrology setup based on the X-ray grating interferometry technique for spatially resolved, quantitative, in situ and at-wavelength measurements of the wavefront at synchrotron radiation and hard X-ray free-electron laser beamlines is reported. Indeed, the ever-increasing demands on the optical components to preserve the wavefront shape and the coherence of the delivered X-ray beam call for more and more sensitive diagnostic instruments. Thanks to its angular sensitivity, X-ray grating interferometry has been established in recent years as an adequate wavefront-sensing technique for quantitatively assessing the quality of the X-ray wavefront under working conditions and hence for the in situ investigation of X-ray optical elements. In order to characterize the optical elements at any given beamline by measuring the aberrations introduced in the wavefront, a transportable X-ray grating interferometry setup was realised at the Swiss Light Source (SLS). The instrument, which is expected to be a valuable tool for investigating the quality of the X-ray beam delivered at an endstation, will be described hereafter in terms of the hardware setup and the related data analysis procedure. Several exemplary experiments performed at the X05DA Optics beamline of the SLS will be presented.

X-ray techniques have evolved over decades to become highly refined tools for a broad range of investigations. Importantly, these approaches rely on X-ray measurements that depend linearly on the number of incident X-ray photons. The advent of X-ray free electron lasers (XFELs) is opening the ability to reach extremely high photon numbers within ultrashort X-ray pulse durations and is leading to a paradigm shift in our ability to explore nonlinear X-ray signals. However, the enormous increase in X-ray peak power is a double-edged sword with new and exciting methods being developed but at the same time well-established techniques proving unreliable. Consequently, accurate knowledge about the threshold for nonlinear X-ray signals is essential. Herein we report an X-ray spectroscopic study that reveals important details on the thresholds for nonlinear X-ray interactions. By varying both the incident X-ray intensity and photon energy, we establish the regimes at which the simplest nonlinear process, two-photon X-ray absorption (TPA), can be observed. From these measurements we can extract the probability of this process as a function of photon energy and confirm both the nature and sub-femtosecond lifetime of the virtual intermediate electronic state., Scientific Reports, 6, ISSN:2045-2322

We report on the temporal pulse characteristics of individual harmonics in an attosecond pulse train by means of photoelectron streaking in a strong low-frequency transient. The scheme allows one to retrieve the pulse durations and first-order chirp of individual harmonics without the need for temporal scanning. The measurements were performed using an intense THz field generated by a tilted phase front technique in ${\mathrm{LiNbO}}_{3}$. We compared the performance of Xe clusters and atomic He as a detection medium and retrieved the temporal properties for harmonics of order 19, 21, 23, 25, and 27. Our measurements confirm that the individual pulse durations and linear chirp decrease by harmonic order.

We have performed femtosecond X-ray spectroscopy measurements after UV photoexcitation of a colloidal solution of ZnO nanoparticles. The results indicate sub-ps hole trapping at oxygen vacancies with shallowly-trapped electrons in the conduction band.

SwissFEL is a free electron laser facility for hard and soft X-rays at the Paul Scherrer Institut in Switzerland. The first hard X-ray FEL named ARAMIS will deliver photons in the wavelength range from 1 A to 7 A in up to three beamlines alternatively. The beamlines are equipped with crystal monochromators, cover the full wavelength range and offer a variety of operational modes.

Picosecond and femtosecond X-ray absorption spectroscopy is used to probe the changes of the solvent shell structure upon electron abstraction of aqueous iodide using an ultrashort laser pulse. The transient L(1,3) edge EXAFS at 50 ps time delay points to the formation of an expanded water cavity around the iodine atom, in good agreement with classical and quantum mechanical/molecular mechanics (QM/MM) molecular dynamics (MD) simulations. These also show that while the hydrogen atoms pointed toward iodide, they predominantly point toward the bulk solvent in the case of iodine, suggesting a hydrophobic behavior. This is further confirmed by quantum chemical (QC) calculations of I(-)/I(0)(H(2)O)(n=1-4) clusters. The L(1) edge sub-picosecond spectra point to the existence of a transient species that is not present at 50 ps. The QC calculations and the QM/MM MD simulations identify this transient species as an I(0)(OH(2)) complex inside the cavity. The simulations show that upon electron abstraction most of the water molecules move away from iodine, while one comes closer to form the complex that lives for 3-4 ps. This time is governed by the reorganization of the main solvation shell, basically the time it takes for the water molecules to reform an H-bond network. Only then is the interaction with the solvation shell strong enough to pull the water molecule of the complex toward the bulk solvent. Overall, much of the behavior at early times is determined by the reorientational dynamics of water molecules and the formation of a complete network of hydrogen bonded molecules in the first solvation shell.

Next-generation X-ray sources, based on the X-ray Free Electron Laser (XFEL) concept, will provide highly coherent, ultrashort pulses of soft and hard X-rays with peak intensity many orders of magnitude above that of a synchrotron. These pulses will allow studies of femtosecond dynamics at nanometer resolution and with chemical selectivity. They will produce coherent-diffraction images of organic and inorganic nanostructures without the deleterious effects of radiation damage.

The Paul Scherrer Institute is planning the construction of an X-ray free electron laser (SwissFEL), which will produce 20-fs pulses of coherent X-rays in the wavelength range 0.1–7 nm, with peak brightness approximately 10 10 times that of a third-generation synchrotron beamline. The brightness, the coherence and the short pulses will provide opportunities for performing novel science in the fields of chemistry, biochemistry, solid-state physics and materials science. It is planned that the SwissFEL will be operational by the end of 2016. The present article focuses on promising SwissFEL applications in the field of time-resolved X-ray scattering from chemical systems.

A new X-ray chopper system based on air-bearing technology was developed in a joint project between the Paul Scherrer Institut and DESY. The X-ray chopper wheel of 150 mm diameter has a slit width of 50 µm, which corresponds to an opening time of 230 ns at 30 000 r min−1. The wheel is equipped with either one or two slits at slightly different radii, resulting in repetition frequencies of 500 and 1000 Hz. To reduce air friction the wheel is operated in a reduced-pressure environment. The chopper is controlled by a specially developed phase lock loop controller, which is synchronized to the master bunch clock of the synchrotron. The very small and constant friction of the bearing and the high mechanical accuracy of all mechanical components in combination with the high-precision controller resulted in a very small long-term jitter of less than 3 ns. The chopper is capable of isolating X-rays generated from a single bunch of the future PETRA III storage ring at DESY operated in 40-bunch mode.

X-ray absorption spectroscopy is a powerful probe of molecular structure, but it has previously been too slow to track the earliest dynamics after photoexcitation. We investigated the ultrafast formation of the lowest quintet state of aqueous iron(II) tris(bipyridine) upon excitation of the singlet metal-to-ligand-charge-transfer ( 1 MLCT) state by femtosecond optical pump/x-ray probe techniques based on x-ray absorption near-edge structure (XANES). By recording the intensity of a characteristic XANES feature as a function of laser pump/x-ray probe time delay, we find that the quintet state is populated in about 150 femtoseconds. The quintet state is further evidenced by its full XANES spectrum recorded at a 300-femtosecond time delay. These results resolve a long-standing issue about the population mechanism of quintet states in iron(II)-based complexes, which we identify as a simple 1 MLCT→ 3 MLCT→ 5 T cascade from the initially excited state. The time scale of the 3 MLCT→ 5 T relaxation corresponds to the period of the iron-nitrogen stretch vibration.

The first tunable undulator source for femtosecond hard X-rays in the range 4–12 keV is now in operation at the SLS storage ring. The source combines accelerator and laser technology relevant for future seeded free electron lasers. It provides inherently synchronized femtosecond laser ‘pump’ and X-ray ‘probe’ pulses to enable time-resolved diffraction and absorption experiments. By using X-ray diffraction to probe laser-induced coherent optical phonons in bulk bismuth, we estimate an X-ray pulse duration of 140 ± 30 fs FWHM with timing drifts below 30 fs rms measured over 5 days. The excellent spatial and temporal stability of the source allows quantitative measurement of ultrafast lattice dynamics and associated phase transitions in real space with atomic resolution and instrumental time resolution of 85 fs rms. Studying semimetals such as bismuth, we have demonstrated (i) grazing incidence femtosecond X-ray diffraction on single crystals that allows us to more completely characterize the ultrafast structural dynamics of solids, and (ii) optical control of real space coherent atomic motion. Both methods will be used to study the dynamics of photo-induced phase transitions in strongly correlated systems such as manganites. The time resolution of such measurements could be improved by one order of magnitude at future XFEL facilities at much higher flux. Femtosecond linear and non-linear resonant X-ray scattering employing full polarization control both in the soft (0.3–3 keV) and hard (4–15 keV) X-ray regime will become feasible which allows direct measurement of orbital degrees of freedom. However, a laser and hard X-ray cross-correlation technique with sufficient temporal resolution and signal-to-noise ratio appropriate for single shot operation has yet to be realized. Again, laser seeding using a phase stabilized few-cycle (5–7 fs) laser may be a viable option to generate

SwissFEL is the Free Electron Laser (FEL) facility under construction at the Paul Scherrer institute (PSI), aiming to provide users with X-ray pulses of lengths down to 2 femtoseconds at standard operation. The measurement of the length of the FEL pulses and their arrival time relative to the experimental laser is crucial for the pump-probe experiments carried out in such facilities. This work presents a new device that measures hard X-ray FEL pulses based on the THz streak camera concept. It describes the prototype setup called pulse arrival and length monitor (PALM) developed at PSI and tested in Spring-8 Angstrom Compact Free Electron Laser (SACLA) in Japan. Based on the first results obtained from the measurements, we introduce the new improved design of the second generation PALM setup that is currently under construction and will be used in SwissFEL photon diagnostics.

The Linac Coherent Light Source has added a self-seeding capability to the soft x-ray range using a grating monochromator system. We report the demonstration of soft x-ray self-seeding with a measured resolving power of 2000–5000, wavelength stability of 10$^{−4}$, and an increase in peak brightness by a factor of 2–5 across the photon energy range of 500–1000 eV. By avoiding the need for a monochromator at the experimental station, the self-seeded beam can deliver as much as 50-fold higher brightness to users.

The accurate measurement of the arrival time of a hard X-ray free electron laser (FEL) pulse with respect to a laser is of utmost importance for pump-probe experiments proposed or carried out at FEL facilities around the world. This manuscript presents the latest device to meet this challenge, a THz streak camera using Xe gas clusters, capable of pulse arrival time measurements with an estimated accuracy of several femtoseconds. An experiment performed at SACLA demonstrates the performance of the device at photon energies between 5 and 10 keV with variable photon beam parameters. (C) 2014 Optical Society of America

The advent of high performance 3rd generation synchrotron sources boosted progress of computer tomographic research towards larger energies and higher resolution. To surpass present limitations in resolution (>1 μm) and efficiency (a few %) proceeding to higher energies, we have developed a innovative technique using 2 extremely asymmetrical Bragg crystals for X-ray imaging and magnification. The device yields distortion and aberration free images and near-field holograms with magnification factors up to 250×250 at X-ray energies around 22 keV with drastically increased efficiency. In conjunction with the X-ray sensing pixel detector PILATUS the total efficiency could be further improved. Thus even at highest magnification factors exposure times of a few msec could be achieved.

The most used detection system in state-of-the-art synchrotron-based microtomography devices usually collects light produced by a thin scintillator and conveys it to charge coupled device (CCD) through a microscope optics. This detection system is intrinsically limited by scintillation properties, optical coupling and CCD granularity to a practical limit of about 1 μ m spatial resolution and efficiency of a few percent. A novel detector, called Bragg magnifier, is a method recently proposed to efficiently exceed the micrometer barrier. It exploits two-dimensional asymmetric Bragg diffraction from flat crystals to produce X-ray images with magnification factors up to 150 × 150 and pixel sizes less than 100 × 100 nm 2 . This work presents its functional principle, some applications and future developments.

The Materials Science Beamline at the Swiss Light Source (SLS) has been designed to produce hard X-rays in the photon-energy range 5–40 keV, at an intermediate energy (2.4 GeV) synchrotron. To this end, it employs a novel “minigap wiggler”. Important issues in the design and realization of the beamline are the high heat load, robust system design, flexibility of operation and user-friendliness. A conventional collimating-mirror/sagittally focusing double-crystal monochromator/focusing mirror optics has been chosen with approximately 1:1 symmetry. Established component designs have been used wherever possible. Three serial end-stations are served with X-rays. Besides the minigap wiggler, other novel or unusual features are: continuous “top-up” injection in the SLS storage-ring, a rotating carbon “cup” filter in the beamline front-end, angles and bending radii of the optics mirrors which are adjusted at each change in photon-energy and special experimental-station equipment including high-speed one- and two-dimensional semiconductor detectors for powder and surface diffraction and a two-dimensional “Bragg magnifier” for tomography. In this work, a comparison is made between predicted and measured beamline properties, and Appendices with useful formulae and algorithms are provided.

We present a setup which allows the measurement of time-resolved x-ray absorption spectra with picosecond temporal resolution on liquid samples at the Advanced Light Source at Lawrence Berkeley National Laboratories. The temporal resolution is limited by the pulse width of the synchrotron source. We characterize the different sources of noise that limit the experiment and present a single-pulse detection scheme.

X-ray computer microtomography is a powerful tool for nondestructive examinations in medicine, biology, and material sciences. The resolution of the presently used detector systems is restricted by scintillator properties, optical light transfer, and charge-coupled-device granularity, which impose a practical limit of about 1 μm spatial resolution at detector efficiencies of a few percent. A recently developed detector, called the Bragg magnifier, achieves a breakthrough in this respect, satisfying the research requirements that ask for an efficient advance towards the submicron range. The Bragg magnifier uses the properties of asymmetric Bragg reflections to increase the cross section of the diffracted x-ray beam. Magnifications of up to 100×100 can be achieved even at hard x-rays energies (>20 keV). In this way, the influence of the detector resolution can be scaled down accordingly and the efficiency increased. Such a device has been developed and successfully integrated into the Microtomography Statio...

Synchrotron-based microtomographic devices are powerful, non-destructive, high-resolution research tools. Highly brilliant and coherent X-rays extend the traditional absorption imaging techniques and enable edge-enhanced and phase-sensitive measurements. At the Materials Science Beamline MS of the Swiss Light Source (SLS), the X-ray microtomographic device is now operative. A high performance detector based on a scintillating screen optically coupled to a CCD camera has been developed and tested. Different configurations are available, covering a field of view ranging from 715×715 μm 2 to 7.15×7.15 mm 2 with magnifications from 4× to 40×. With the highest magnification 480 lp/mm had been achieved at 10% modulation transfer function which corresponds to a spatial resolution of 1.04 μm. A low-noise fast-readout CCD camera transfers 2048×2048 pixels within 100–250 ms at a dynamic range of 12–14 bit to the file server. A user-friendly graphical interface gives access to the main parameters needed for running a complete tomographic scan. This novel device will be used to study the physical structure and chemical composition of biological and technical materials, e.g. enabling pseudo-dynamic testing of bone samples to establish structure–function relationships in simulated osteoporosis or enabling non-destructive testing during the development of modern composite materials.

The insertion devices under construction for phase I of the Swiss Light Source (SLS) are described. Five undulators and one wiggler will be installed in four straight sections of the third generation 2.4 GeV SLS storage ring, under construction at the Paul Scherrer Institute. To provide undulator radiation in the energy range from 10 eV to 18 keV , both long period and short period, small gap undulators will be installed.

The conceptual designs for the insertion device front ends [1] have been completed for the 2.4 GeV swiss light source (SLS), currently under construction at the Paul Scherrer Institute. The critical component of the front ends, the photon shutter, has been designed to be capable of absorbing the full intensity of the photon beams from the insertion devices [2] . In this contribution, the detailed shutter design will be discussed. The thermal and structural analysis results obtained from a finite element calculation for the Material Science Beamline 4S [3] , which produces the highest power load at the shutter (4 kW, 95 W/mm 2 ) of all the SLS beamlines, will be presented. A test using an electron beam welding machine to simulate the photon beam source will be described. The experimental results are compared with those from finite element calculations, and they confirm that the designed shutter can be safely operated in the front end of beamline 4S.

We describe the “Surface/Interface: Microscopy” beamline currently under construction at the Paul Scherrer Institut. This beamline will use a photoemission electron microscope to study the electronic and magnetic structure of materials. Its photon energy range will be 94–2000 eV. To allow time resolved measurements with millisecond resolution we use a new scheme allowing to switch the photon helicity optically without perturbing the electron orbit. Two identical elliptical insertion devices are placed behind each other in the same straight section. They can produce light with opposing helicities. These two sources are separated horizontally by introducing a small static parallel offset in the electron orbit. Switching between the two rays of opposite helicities is done mechanically at the horizontal focus behind the monochromator. The two sources are brought to overlap on the sample by slightly defocussing the refocussing mirror. A commercial microscope ( Δx ∼20 nm resolution) is adapted to the synchrotron by various upgrades. These include a software combining microscope and beamline control, a computer controlled mechanical alignment system, a separate sample preparation chamber, and sample cooling using liquid nitrogen. The beamline will be available for user operation in 2002.

We present a picosecond Fe K-edge absorption study of photoexcited ferrous and ferric hexacyanide in water under 355 and 266 nm excitation. Following 355 nm excitation, the transient spectra for the ferrous and ferric complexes exhibit a red shift of the edge reflecting an increased electron density at the Fe atom. For the former, an enhanced pre-edge transition is also observed. These observations are attributed to the aquated [Fe(CN)5OH2]3− species, based on quantum chemical calculations which also provide structural parameters. Upon 266 nm excitation of the ferric complex, a transient reminiscent of the aquated species is observed (appearance of a pre-edge feature and red shift of the edge) but it is different from that obtained under 355 nm excitation. This points to a new reaction channel occurring through an intermediate state lying between these two excitation energies. Finally, 266 nm excitation of the ferrous species is dominated by the photooxidation channel with formation of the ferric complex as main photoproduct. However, we observe an additional minor photoproduct, which is identical to the 266 nm generated photoproduct of the ferric species, suggesting that under our experimental conditions, the pump pulse photooxidises the ferrous complex and re-excites the primary ferric photoproduct.

A technique has been tested for the first time which combines the advantages of continuous and pulsed muon beams, namely high time resolution and low background in time-differential μSR experiments. In addition, the method allows the muon beam to be split and two μSR experiments run simultaneously at full intensity without any interference between the instruments.

The $({\ensuremath{\pi}}^{+},{\ensuremath{\pi}}^{\ensuremath{-}})$ reaction on the isoscalar, doubly magic nuclei ${}^{16}\mathrm{O}$ and ${}^{40}\mathrm{Ca}$ has been measured in the energy range ${T}_{\ensuremath{\pi}}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}45--90\mathrm{MeV}$. The forward angle cross sections of the ground state transitions (GST) show a very pronounced resonancelike energy dependence. The observed energy and angle dependences are well described by the recent hypothesis of the formation of a $\ensuremath{\pi}\mathrm{NN}$ resonance in the course of the double charge exchange process. The deduced spreading widths are in accordance with estimates of the ${d}^{\ensuremath{'}}$ collision damping in the nuclear medium. In the reaction on ${}^{16}\mathrm{O}$ in addition to the GST the transition to a ${0}^{+}$ state at ${E}_{x}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}2.1(2)\mathrm{MeV}$ in ${}^{16}\mathrm{Ne}$ has been observed, which is interpreted as the quadruple isobaric analog state (QIAS) of the ${0}_{2}^{+}$ state in ${}^{16}\mathrm{C}$ at ${E}_{x}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}3.03\mathrm{MeV}$.

After the successful demonstration of the hard X-ray self-seeding at LCLS, an effort to build a system for working in the soft X-ray region is ongoing. The idea for self-seeding in the soft X-ray region by using a grating monochromator was first proposed by Feldhauset. al. The concept places a grating monochromator in middle of the undulators and selects a narrow bandwidth “seed” from the SASE beam produced by the upstream section of undulators, which is then amplified to saturation in the downstream section of the undulators. The seeded FEL beam will have a narrower bandwidth approaching the transform limit. The challenge is to accommodate a monochromator and refocusing system as well as the electron beam magnetic chicane into a very limited space. The Soft X-raySelf Seeding system replaces only a single undulator section of ~ 4 m. Theoverall project and the expected FEL performances are described elsewhere. Here we present the detailed optical design solution, consisting of a fixed incidence angle toroidal blazed grating with variable groove density, a rotating plane mirror (the only required motion for tuning the energy) to redirect the selected monochromatic beam onto an exit slit, and two more mirrors, one sphere and one flat, to focus and overlap the ‘seed’ onto the electron beam in the downstream undulators.

Knowledge of the structure of biological macromolecules, especially in their native environment, is crucial because of the close structure–function relationship. X-ray small-angle scattering is used to determine the shape of particles in solution, but the achievable resolution is limited owing to averaging over particle orientations. In 1977, Kam proposed to obtain additional structural information from the cross-correlation of the scattering intensities. Here we develop the method in two dimensions, and give a procedure by which the single-particle diffraction pattern is extracted in a model-independent way from the correlations. We demonstrate its application to a large set of synchrotron X-ray scattering images on ensembles of identical, randomly oriented particles of 350 or 200 nm in size. The obtained 15 nm resolution in the reconstructed shape is independent of the number of scatterers. The results are discussed in view of proposed ‘snapshot’ scattering by molecules in the liquid phase at X-ray free-electron lasers.

A position sensitive detector for 3–30 keV positrons and electrons has been developed which consists of a pair of microchannel plates (MCP) in Chevron configuration and resistive anode readout. The device has an active diameter of 75 mm and can be operated in axial magnetic fields up to several kG. The detection efficiency of MCP devices is 16(2)% for positrons in the 10 keV region. With a thin carbon (C) foil of 25 μg/cm 2 thickness carrying a 15 μg/cm 2 magnesium oxide (MgO) coating acting as additional secondary electron emitter, the efficiency could be increased to 64(2)% in the energy range 5–12 keV. A two-dimensional position resolution of 0.55(3) mm (FWHM) and a timing resolution of better than 1 ns could be achieved.